Abstract In optical materials energy is usually extracted only from the lowest excited state, resulting in fundamental energy-efficiency limits such as the Shockley–Queisser limit for single-junction solar cells. Photon-cutting materials provide a way around such limits by absorbing high-energy photons and ‘cutting’ them into multiple low-energy excitations that can subsequently be extracted. The occurrence of photon cutting or quantum cutting has been demonstrated in a variety of materials, including semiconductor quantum dots, lanthanides and organic dyes. Here we show that photon cutting results in bunched photon emission on the timescale of the excited-state lifetime, even when observing a macroscopic number of optical centres. Our theoretical derivation matches well with experimental data on NaLaF4:Pr3+, a material that can cut deep-ultraviolet photons into two visible photons. This signature of photon cutting can be used to identify and characterize new photon-cutting materials unambiguously.
Abstract In optical materials energy is usually extracted only from the lowest excited state, resulting in fundamental energy-efficiency limits such as the Shockley–Queisser limit for single-junction solar cells. Photon-cutting materials provide a way around such limits by absorbing high-energy photons and ‘cutting’ them into multiple low-energy excitations that can subsequently be extracted. The occurrence of photon cutting or quantum cutting has been demonstrated in a variety of materials, including semiconductor quantum dots, lanthanides and organic dyes. Here we show that photon cutting results in bunched photon emission on the timescale of the excited-state lifetime, even when observing a macroscopic number of optical centres. Our theoretical derivation matches well with experimental data on NaLaF4:Pr3+, a material that can cut deep-ultraviolet photons into two visible photons. This signature of photon cutting can be used to identify and characterize new photon-cutting materials unambiguously.
High Resolution Image Download MS PowerPoint Slide Spectral conversion of sunlight can enhance solar cell efficiencies by shifting short-wavelength photons to longer wavelengths, where the photovoltaic response is stronger. This can be realized with near 100% energy efficiency by materials capable of quantum cutting . These emit two longer-wavelength photons, following the absorption of one shorter-wavelength photon. Although various quantum-cutting materials have been reported, follow-up research has often disproved initial claims. Here, we demonstrate that photon correlation analysis is a universal strategy to unambiguously identify quantum cutting. We investigate two materials, YPO 4 codoped with Tb 3+ and Yb 3+ and yttrium aluminum garnet (YAG) codoped with Ce 3+ and Yb 3+ . Both are reported to perform quantum cutting via blue light absorption followed by cooperative energy transfer to near-infrared-emitting Yb 3+, but some studies have cast doubts for YAG:Ce 3+,Yb 3+ . Our correlation analysis demonstrates bunched emission for YPO 4:Tb 3+,Yb 3+, confirming quantum cutting. In contrast, YAG:Ce 3+,Yb 3+ shows Poissonian emission statistics, disproving its quantum-cutting capability, despite previous claims.
Even though the quantized interaction between light and matter in the photoelectric effect is considered one of the cornerstones in the development of quantum mechanics, it was long thought impossible to directly observe the quantized nature of light itself. The advent of light-intensity autocorrelation techniques in the 1950s, first developed to study the size of stars, changed little in this perception, until true single-photon correlation spectroscopy from trapped ions was proven to be possible in the late 1970s: Photons from a single quantum emitter tend to arrive in bunches, but each light quantum is spaced apart in time—it is antibunched. Initially considered only as the workhorse of atomic quantum optics, over the past two decades, photon correlation techniques have become a standard in fields as diverse as quantum-information processing, biological imaging, polymer physics, and materials science, in general. The technique is particularly useful for probing materials that are specifically designed to emit or absorb light in optoelectronic devices, such as light-emitting diodes, solar cells, or lasers. The central question in such studies is how large a mesoscopic piece of material can become and still behave as an atom-like source of single photons. What interactions may arise between multiple excitations within a material, and what sort of dark states may give rise to intermittency in the stream of photons? We review the many different classes of optoelectronic materials for which photon-correlation spectroscopy has proven to offer useful insight into excited-state dynamics, ranging from molecular, over semiconductor to metallic nanostructures. The technique is particularly suited to probing mesoscopic aggregates of organic semiconductors since each single molecule acts as a quantum emitter itself.
We investigate the intensity correlation properties of single photons emitted from an optically excited single semiconductor quantum dot. The second order temporal coherence function of the photons emitted at various wavelengths is measured as a function of the excitation power. We show experimentally and theoretically that a quantum dot is not only a source of nonclassically correlated monochromatic photons but is also a source of multicolor photons with tunable correlation properties. We found that the emitted photon statistics can be varied by the excitation rate from a sub-Poissonian one, where the photons are temporally antibunched, to super-Poissonian, where they are temporally bunched.
Shot noise sets a fundamental limit on the sensitivity of classical optical measurements, with coherent emitters achieving the lowest possible shot-noise level. Emission from sub-Poissonian light provides a pathway to surpass this limit, and single-photon sources provide a natural platform for generating such light. However, it is commonly assumed that continuously excited single-photon sources exhibit Poissonian statistics. In this work, a theoretical model of a continuously driven two-level single-photon source is developed, treating both excitation and radiative decay as stochastic processes. The analysis demonstrates that photon emission can display sub-Poissonian statistics when excitation and decay rates are comparable, showing that continuous excitation does not inherently preclude nonclassical emission. The model is further extended to include finite detection efficiency and detector dead time, illustrating how these practical non-idealities can affect the experimental observation of sub-Poissonian statistics.
We present a combined experimental and theoretical study of two-photon emission from the biexciton cascade in single GaN quantum dots. By changing the biexciton binding energy, pump power, and temperature, the balance between the one- and two-photon decay processes is controlled in this four-level system, which drastically affects the photon statistics of the resulting emission. As the most pronounced feature of this interplay we observe a bunching phenomenon and a transition from sub- to super-Poissonian photon statistics, originating from the complex nature of the biexciton cascade. This work highlights how photon statistics can be steered between one- and two-photon processes towards an increased, bunched two-photon emission probability up to 50 K with the perspective for efficient photon pair generation in the UV spectral range.
Photon anti-bunching is the direct evidence for the existence of photons without having a classical counterpart. Unlike bunching of photons, which can have a semi-classical description, the effect of photon anti-bunching can only be understood with quantized electromagnetic fields. However, for the process of high harmonic generation (HHG), where many photons of the driving field are upconverted to a single photon of higher energy, there is yet no clear evidence for the presence of individual photon emission. The key result of this work is the prediction of photon anti-bunching in the process of HHG, marking it the first theoretical discovery of non-classicality in the temporal correlations of HHG photons. While other non-classical signatures in HHG, such as sub-Poissonian statistics or squeezing, have been discussed for an ensemble of photons, the anti-bunching signature reported here is a signature of a single photon. This is achieved by using the recently developed Heisenberg picture approach for quantum optical HHG, revealing clear anti-bunching signatures in the intensity correlation function across the entire harmonic spectrum.